Coke-resistant Au-Ni/MgAl2O4 catalyst for direct methanation of syngas

能源化学(英文版) ›› 2019, Vol. 39 ›› Issue (12): 198-207.

Coke-resistant Au-Ni/MgAl₂O₄ catalyst for direct methanation of syngas

Fen Wang^a,b, Jing-Cai Zhang^b,c, Wei-Zhen Li^b,c, Bing-Hui Chen^a

a National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China;
b Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
c Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China

收稿日期:2018-12-31 修回日期:2019-03-04 出版日期:2019-12-15 发布日期:2020-12-18
通讯作者: Wei-Zhen Li, weizhenli@dicp.ac.cn; Bing-Hui Chen, chenbh@xmu.edu.cn
基金资助:
This work was supported by the National Key R&D Program of China (2016YFA0202801), the National Natural Science Foundation of China (21673226, 21673187), the "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21040200).

Coke-resistant Au-Ni/MgAl₂O₄ catalyst for direct methanation of syngas

Fen Wang^a,b, Jing-Cai Zhang^b,c, Wei-Zhen Li^b,c, Bing-Hui Chen^a

a National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, Department of Chemical and Biochemical Engineering, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian, China;
b Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, Liaoning, China;
c Dalian National Laboratory for Clean Energy, Dalian 116023, Liaoning, China

Received:2018-12-31 Revised:2019-03-04 Online:2019-12-15 Published:2020-12-18
Contact: Wei-Zhen Li, weizhenli@dicp.ac.cn; Bing-Hui Chen, chenbh@xmu.edu.cn
Supported by:
This work was supported by the National Key R&D Program of China (2016YFA0202801), the National Natural Science Foundation of China (21673226, 21673187), the "Transformational Technologies for Clean Energy and Demonstration", Strategic Priority Research Program of the Chinese Academy of Sciences (XDA21040200).

摘要/Abstract

摘要： Carbon deposition is one of the major issues for catalytic methanation, especially when using high CO content syngas (such as H₂/CO=1) due to the inevitable Boudouard reaction. Here we report the significant enhancement on the coke-resistance of Ni/MgAl₂O₄ catalyst during methanation by modifying with Au. The coke-resistant property was increased with Au addition while the catalytic activity decreased with excess Au. High and stable syngas conversions can be obtained over Au-Ni/MgAl₂O₄ catalyst at 450-500℃. With comprehensive characterizations by using BET, H₂ chemisorption, H₂-TPR, XPS, XRD, STEM, EDS, TEM, TG/DTA, Raman and TPH, we found that Au and Ni formed bimetallic nanoparticles of ～10 nm with electron donation from Ni to Au. The deposited carbon on the spent Au-Ni/MgAl₂O₄ is very similar to that on the spent Ni/MgAl₂O₄ in the nature and in the gasification behaviour but is significantly less. These results suggest that the enhanced coke-resistance of Au-Ni/MgAl₂O₄ is presumably due to the suppression on CO disproportionation by modifying Ni with Au.

关键词: Syngas, Methanation, Methane, Coke resistance, Ni catalyst, Gold

Abstract: Carbon deposition is one of the major issues for catalytic methanation, especially when using high CO content syngas (such as H₂/CO=1) due to the inevitable Boudouard reaction. Here we report the significant enhancement on the coke-resistance of Ni/MgAl₂O₄ catalyst during methanation by modifying with Au. The coke-resistant property was increased with Au addition while the catalytic activity decreased with excess Au. High and stable syngas conversions can be obtained over Au-Ni/MgAl₂O₄ catalyst at 450-500℃. With comprehensive characterizations by using BET, H₂ chemisorption, H₂-TPR, XPS, XRD, STEM, EDS, TEM, TG/DTA, Raman and TPH, we found that Au and Ni formed bimetallic nanoparticles of ～10 nm with electron donation from Ni to Au. The deposited carbon on the spent Au-Ni/MgAl₂O₄ is very similar to that on the spent Ni/MgAl₂O₄ in the nature and in the gasification behaviour but is significantly less. These results suggest that the enhanced coke-resistance of Au-Ni/MgAl₂O₄ is presumably due to the suppression on CO disproportionation by modifying Ni with Au.

Key words: Syngas, Methanation, Methane, Coke resistance, Ni catalyst, Gold

Fen Wang, Jing-Cai Zhang, Wei-Zhen Li, Bing-Hui Chen. Coke-resistant Au-Ni/MgAl₂O₄ catalyst for direct methanation of syngas[J]. 能源化学(英文版), 2019, 39(12): 198-207.

Fen Wang, Jing-Cai Zhang, Wei-Zhen Li, Bing-Hui Chen. Coke-resistant Au-Ni/MgAl₂O₄ catalyst for direct methanation of syngas[J]. Journal of Energy Chemistry, 2019, 39(12): 198-207.

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Coke-resistant Au-Ni/MgAl₂O₄ catalyst for direct methanation of syngas

Coke-resistant Au-Ni/MgAl₂O₄ catalyst for direct methanation of syngas

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